Contrib Mineral Petrol (2014) 167:966

DOI 10.1007/s00410-014-0966-x

ORIGINAL PAPER

Intermittent mixing processes occurring before Plinian eruptions

of Popocatepetl volcano, Mexico: insights from textural
compositional variations in plagioclase and SrNdPb isotopes
G. Sosa-Ceballos J. E. Gardner J. C. Lassiter

Received: 14 January 2012 / Accepted: 9 January 2014 / Published online: 29 January 2014
Springer-Verlag Berlin Heidelberg 2014

Abstract Volcan Popocatepetl has explosively erupted in

Plinian style at least five times in the last 23,000 years.
Extreme deviations in composition and the occurrence of
dissolution features in plagioclase and pyroxene, and the
occasional presence of xenocrysts of Cr-rich FeTi oxides
and Mg-rich olivines and pyroxenes indicate that magma
mixing has been a major process affecting the magmatic
system. The nearly invariant composition of the erupted
products (andesiticdacitic) suggests, however, that mixing
is not acting alone and must be balanced by assimilation
and/or crystallization. To investigate the magmatic processes that have modified the Plinian magmas, textural and
compositional variations and growth rates in plagioclase
were used to approximate the frequency of mixing events
affecting each magma. Systematic analysis of Sr, Nd, and
Pb isotopes was carried out on plagioclase, pyroxene, and
pumice matrix glass to constrain the extent of assimilation
of upper crustal rocks. Additionally, a series of phase
equilibrium experiments were carried out to constrain the
depth where such mixing and assimilation occurred. We
Communicated by G. Moore.

Electronic supplementary material The online version of this

article (doi:10.1007/s00410-014-0966-x) contains supplementary
material, which is available to authorized users.
Present Address:
G. Sosa-Ceballos (&)  J. E. Gardner  J. C. Lassiter
Department of Geological Sciences, Jackson School of
Geosciences, The University of Texas at Austin,
Austin, TX, USA
e-mail: gsosaceballos@gmail.com;
giovanni@geofisica.unam.mx
G. Sosa-Ceballos
Instituto de Geofsica, Campus Morelia, Universidad Nacional
Autonoma de Mexico, Morelia, Michoacan, Mexico

find that magma was stored at one of two different depths

beneath Popocatepetl with magma mixing acting in both
reservoirs. Mixing frequency and the relative impact on
mineral compositions and textures has varied with time.
Assimilation of calcareous rocks underneath Popocatepetl
has not been pervasive and does not contribute significantly
to the evolution of the Plinian magmas. The similar compositions of magmas with diverse mixing histories suggest
that fractional crystallization, and possibly assimilation of
deep crust, takes place at depth and that intermediate
magmas ascend into the upper crust already differentiated.
Keywords Popocatepetl  Magma mixing  Plagioclase 
Phase equilibrium experiments  Radiogenic isotopes

Introduction
Fractional crystallization of basaltic magma contributes
greatly to the generation of calc-alkaline magma in subduction zones (e.g., Heiken and Eichelberger 1980; Singer
et al. 1995). Mixing of magmas and assimilation of crustal
rocks must also contribute, however, in order to explain the
wide diversity of bulk isotopic compositions of intermediate-silicic magmas and the disequilibrium textures in
their minerals (e.g., De Paolo 1981; Sisson and Grove
1993; Gardner et al. 1995a, b; Clynne 1999; Tepley et al.
2000; Couch et al. 2001; Annen et al. 2006; Bohrson and
Spera 2007; Brophy 2009). The occurrence of mixing and
assimilation is indisputable, but how often such events
occur and how much they affect the composition and texture of crystals in any single magma body are poorly
constrained. In addition, because mixing has been linked as
a potential trigger for eruptions worldwide, it is of interest
to know whether such events occur similarly before Plinian

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eruptions, especially at volcanoes that do not erupt frequently in Plinian fashion.

One way to determine those frequencies and intensities
is to track systematic records of those processes in a
sequence of magmas tapped by multiple Plinian eruptions.
Two common methods used to evaluate such records
involve measuring variations in SrNdPb isotopic compositions and variations in plagioclase composition (e.g.,
De Paolo 1981; Tepley et al. 2000; Davidson et al. 2001;
Bohrson and Spera 2007; Andrews et al. 2008). Plagioclase
is particularly suited for investigating magmatic processes
because of its extensive thermal stability, its slow internal
diffusive re-equilibration (Morse 1984; Zellmer et al. 1999;
Costa et al. 2003), and its composition reflects variations in
intensive parameters (e.g., Tepley et al. 2000; Couch et al.
2001; Humphreys et al. 2006; Berlo et al. 2007; Andrews
et al. 2008).
Magmas erupted at Popocatepetl volcano, Mexico,
exhibit evidence that mixing between silicic and more
mafic magmas is common (e.g., Straub and Martin DelPozzo 2001; Witter et al. 2005; Schaaf et al. 2005; Atlas
et al. 2006; Roberge et al. 2009; Arana-Salinas et al. 2010;
Sosa-Ceballos et al. 2012). If such mixing were volumetrically significant, however, erupted magmas should progressively become more mafic with time. But, at least for
magmas erupted in Plinian events over the past 23 ky, the
dominant type is intermediate in composition, with no
apparent long-term shift to more mafic compositions (e.g.,
Schaaf et al. 2005; Sosa-Ceballos 2006; Arana-Salinas
et al. 2010). The question thus becomes, does crustal
assimilation or fractional crystallization (or both) tend to
balance injections of mafic magma, with small variations in
composition reflecting differences in their frequency
through time, or does mixing act alone, but is insufficient in
magnitude to significantly alter bulk composition through
time?
In this study, we investigate the magmatic processes
responsible for the evolution of magmas tapped during the
Plinian eruptions at Popocatepetl volcano. In particular, we
seek to know whether the record of the magmatic processes
is similar before each Plinian event. Although such eruptions are relatively rare, they invariably tap magmas with
bulk compositions similar to recent ash emissions (Straub
and Martin Del-Pozzo 2001), as well as lavas that built the
present-day cone (Sosa-Ceballos 2006). The record of
magmatic processes is inferred from textural and compositional analyses of plagioclase and analyses of Sr, Nd, and
Pb isotopes in plagioclase, pyroxene, and pumice matrix
glass (silicate melt). In addition, the relative pre-eruptive
storage conditions under which those processes occur are
constrained through phase equilibrium experiments.
Results show that over the last 23 ky, magmas erupted in
Plinian fashion were variably modified by replenishment of

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Contrib Mineral Petrol (2014) 167:966

mafic magma at one of two depths. The magnitude of those

replenishments appears relatively constant, but their frequency varies significantly. Assimilation of local calcareous rocks is negligible, leaving fractional crystallization
and possibly assimilation of lower crust as the processes
most likely balancing mixing to maintain the relatively
invariant bulk composition.

Geologic background
Popocatepetl volcano, located in the central portion of the
Trans-Mexican Volcanic Belt and related to subduction of
the Cocos plate beneath North America, has had at least
three constructiondestruction periods (Siebe et al. 1995;
Sosa-Ceballos et al. 2012). The age of the first collapse that
destroyed the oldest paleostructure, as described by Mooser
et al. (1958), is unknown. The second edifice was destroyed
by a massive sector collapse *23,000 years ago, as dated
by the associated White pumice Plinian deposit (WP)
(Fig. 1; Siebe et al. 1995). The third destructive event
(caldera collapse) occurred *14,100 years ago during the
Tutti Frutti Plinian Eruption (TFPE). This eruption, composed of the Milky Tephra (MT) and Gray Tephra (GT),
resulted in the formation of a small caldera on the NW
flank of the volcano (Sosa-Ceballos et al. 2012). Since
then, there have been at least three other Plinian eruptions.
Siebe et al. (1996) named these deposits as Upper PreCeramic, Lower Ceramic, and Upper Ceramic. Here, we
use their respective informal names: Ochre Pumice (OP)
(Espinasa-Perena and Martn-Del Pozzo 2006; AranaSalinas et al. 2010); Lorenzo Pumice (LP); and Pink
Pumice (PP) (Fig. 1).
Previous studies have related to the full spectrum of
magmas erupted at Popocatepetl to generation in the
mantle wedge, resulting from dehydration of the subducting slab, followed by fractional crystallization during
ascent and mixingassimilation during stagnation in shallow magma reservoirs (e.g., Straub and Martin Del-Pozzo
2001; Schaaf et al. 2005). Emphasis has been placed on
recharge and pre-eruptive mixing between mafic and silicic
magmas to produce andesites (Nixon and Pearce 1987;
Pearce and Kolisnik 1990; Straub and Martin Del-Pozzo
2001; Schaaf et al. 2005; Witter et al. 2005; Atlas et al.
2006) and on the assimilation of local Cretaceous limestones and Tertiary terrigenous rocks (Goff et al. 2001;
Siebe et al. 2004).
Samples and analytical methods
Large pumice fragments collected from the six Plinian
deposits (WP, MT, GT, OP, LP, and PP) were broken into
three pieces, one of which was used for whole-rock

Contrib Mineral Petrol (2014) 167:966

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966

Table 1 Bulk composition of magmas in wt%

WP

GT

MT

OP

LP

PP

SiO2

64.81

60.55

61.36

62.55

62.07

TiO2

0.81

0.82

0.81

0.82

0.81

62.70
0.81

Al2O3

16.63

16.82

17.04

17.28

16.53

16.16

FeO*

4.16

5.20

5.07

4.84

4.87

5.28

MnO

0.10

0.10

0.10

0.10

0.10

0.10

MgO

2.33

4.59

3.96

2.88

4.46

3.46

CaO

4.36

5.91

5.88

5.04

5.07

4.88

Na2O

3.96

4.08

3.96

4.42

4.16

4.37

K2O

2.64

1.73

1.62

1.85

1.72

2.03

P2O5
Total

0.20
100

0.20
100

0.20
100

0.21
100

0.20
100

0.20
100

Analytical precision (2 SD) average 0.38 wt% SiO2, 0.03 wt% TiO2,
0.33 wt% Al2O3, 0.13 wt% FeO, 0.37 wt% MgO, 0.12 wt% CaO, 0.09
wt% Na2O, 0.04 wt% K2O, 0.02 wt% P2O5

Fig. 1 Composite stratigraphic column of Plinian deposits of Popocatepetl volcano: White Pumice (WP), Tutti Frutti Plinian Eruption
(Gray Tephra (GT) and Main Tephra (MT), Ocher Pumice (OP),
Lorenzo Pumice (LP), and Pink Pumice (PP)). Radiocarbon ages are
from Siebe et al. (1995, 1996), Arana-Salinas et al. (2010), and SosaCeballos et al. (2012). Mineralogies are pl plagioclase, px pyroxene,
ox FeTi oxides, and amp amphibole. Pre-eruptive temperature and
oxygen fugacity (given as the relative difference from the NiNiO
buffer curve) are derived from magnetiteilmenite and/or amphibole
compositions. Oxygen fugacity was not determined for LP

compositional analysis, one for thin sectioning, and the last

for mineral separation. Mounts of 132 plagioclase phenocrysts (an average of 20 per deposit) were made. Parts of
the OP, MT, and WP fragments used for bulk analysis were
also crushed and ground for use in phase equilibrium
experiments. Whole-rock compositions were analyzed at
the GeoAnalytical Laboratory at Washington State University using x-ray fluorescence (XRF).
Major elements in plagioclase, clinopyroxene, orthopyroxene, hornblende, FeTi oxides, and groundmass glass
were analyzed using a JEOL JXA-8600 Electron Microprobe (EPMA) housed in the Department of Geological
Sciences at The University of Texas at Austin. Analyses
were made using 15 keV accelerating voltage and 10 nA
beam current. The beam was focused to analyze plagioclase, pyroxenes, and FeTi oxides, but was defocused to
5 lm to analyze hornblende and to 10 lm to analyze
groundmass glass, in order to avoid water loss and sodium
migration. Detailed textural analyses and core-to-rim
compositional transects across plagioclase were made in

steps of 10 lm with the electron microprobe, except for

those in GT, whose internal sieved texture made it
impossible to analyze uninterrupted transects. Errors
(2r) on plagioclase analyses during the course of this
study average 2 mol% An content.
Sr, Nd, and Pb isotopic compositions of plagioclase,
clinopyroxene, and groundmass glass concentrates were
measured by thermal ionization mass spectrometry (TIMS)
at the University of Texas at Austin, Department of Geological Sciences, using a ThermoFisher TRITON. All
samples were first leached with hot 6 N HCl to remove
superficial contamination. Crystals coated by a fine film of
matrix glass were slightly etched with HF and then cleaned
with water in a sonic bath. Chemical separations of Sr, Nd,
and Pb were accomplished using standard ion-exchange
column techniques, similar to those outlined in Lassiter
et al. (2003), with the exception that: (1) Sr was separated
by using Sr-Spec resin; and (2) rare earth elements (REEs)
were separated using RE-Spec resin, followed by Nd separations using glass columns filled with hydrogen di-ethylhexyl-phosphate resin (HDEHP). Pb separations were
performed using Teflon columns and anion exchange resin.
Experimental methods
Ten grams each of OP, MT, and WP pumice clasts were
ground to fine powders for use in phase equilibrium
experiments. All experiments were run in Ag70Pd30 capsules (2 or 5 mm in diameter) in cold-seal pressure vessels
made of either Waspaloy (experiments B900 C) or TZM
metal (experiments [900 C).
For those runs in Waspaloy pressure vessels, capsules
were welded at one end and starting material and distilled
water were added. Sufficient water was added to ensure

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Contrib Mineral Petrol (2014) 167:966

Table 2 Average composition of most common glass, and phenocrysts rims tapped by the Plinian eruptions at Popocatepetl
SiO2
(wt%)

TiO2
(wt%)

Al2O3
(wt%)

FeO*
(wt%)

MnO
(wt%)

MgO
(wt%)

CaO
(wt%)

Na2O
(wt%)

K2O
(wt %)

Cr2O3
(wt%)

Total
(wt%)

WP
Gl

69.10

Plg

55.94

Am

44.90

Cpx

52.20

Opx

53.73

Mt
Il

n.a.
n.a.

0.42

14.78

2.79

0.05

28.05

0.34

n.a.

n.a.

2.50

9.50

12.90

0.20

0.30

1.70

12.30

0.40

0.09

0.97

19.47

8.66
35.30

3.27
0.51

n.a.

0.73

2.98

5.07

3.22

n.a.

99.10

15

9.88

5.33

0.28

n.a.

99.82

10

14.10

11.00

2.20

0.70

n.a.

98.00

20

13.40

19.90

0.60

0.00

n.a.

100.80

10

0.74

24.83

0.98

0.09

n.d.

n.a.

100.90

10

80.78
59.15

0.33
0.22

2.35
2.32

n.a.
n.a.

n.a.
n.a.

0.35
0.25

95.74
97.76

10
10

17.21

4.28

0.07

25.81

0.29

n.a.

n.a.

n.a.
n.a.

MT
Gl

63.10

Plg

58.10

0.62
n.a.

2.24

5.44

4.49

1.74

n.a.

99.21

12

8.39

6.41

0.44

n.a.

99.40

10
10

Cpx

52.24

0.47

1.78

8.03

0.30

15.26

21.34

0.43

n.d.

n.a.

99.84

Opx

55.18

0.07

0.94

13.01

0.30

28.43

1.31

0.00

n.d.

n.a.

99.25

12

Mt

n.a.

8.10

3.90

83.70

0.50

2.50

n.a.

n.a.

n.a.

n.a.

98.70

10

Il

n.a.

44.40

0.90

47.40

0.30

5.30

n.a.

n.a.

n.a.

0.80

99.10

10

0.60

18.95

4.85

0.02

1.17

4.83

5.08

2.20

n.a.

99.90

15
13

GT
Gl

62.20

Plg

48.30

32.20

0.50

n.a.

n.a.

15.30

2.80

0.10

n.a.

99.20

Am

43.00

2.90

12.10

10.50

0.10

15.30

11.00

2.70

0.50

n.a.

98.10

15

Cpx

51.40

0.83

3.56

7.68

0.18

14.98

20.21

0.50

n.d.

n.a.

99.34

10

Opx

53.60

0.27

1.58

15.55

0.29

27.39

1.31

0.04

n.d.

n.a.

100.02

10

Mt
Il

n.a.
n.a.

10.70
44.10

3.60
0.80

80.30
49.70

0.40
0.50

3.50
4.30

n.a.
n.a.

n.a.
n.a.

0.50
0.00

99.00
99.40

10
10

n.a.

n.a.
n.a.

OP
Gl

68.64

Plg

54.98

Cpx

52.14

Opx

53.56

0.56

15.75

3.12

0.06

2.84

4.67

2.57

n.a.

99.03

13

26.82

0.48

n.a.

n.a.

10.11

5.42

0.25

n.a.

98.05

15

0.47

2.31

9.17

0.34

14.58

21.00

0.56

n.d.

n.a.

100.56

10

1.47

n.a.

0.83

0.24

1.31

18.86

0.45

24.98

0.00

n.d.

n.a.

100.87

10

vMt

n.a.

13.11

1.84

78.54

0.39

2.24

n.a.

n.a.

n.a.

0.29

96.40

10

Il

n.a.

44.32

0.25

51.52

0.44

3.19

n.a.

n.a.

n.a.

0.10

99.82

10

15.80

5.06

0.07

4.08

4.25

2.33

n.a.

99.78

10

25.69

0.48

n.a.

n.a.

10.21

4.57

0.18

n.a.

98.78

9
10

LP
Gl

65.59

Plg

57.67

0.99
n.a.

1.62

Cpx

52.08

0.43

2.82

5.27

0.09

16.06

20.51

0.46

n.d.

n.a.

97.73

Opx

53.49

0.32

1.26

19.79

0.45

23.95

1.39

0.04

n.d.

n.a.

100.69

10

Mt

n.a.

6.73

2.81

84.06

0.29

1.96

n.a.

n.a.

n.a.

0.35

96.20

10

Il

n.a.

47.35

0.43

45.18

0.30

5.30

n.a.

n.a.

n.a.

0.60

99.15

10

15.85

3.11

0.08

26.31

0.44

n.a.

PP
Gl
Plg

67.07
55.85

0.75
n.a.

1.13
n.a.

3.41

4.38

2.83

n.a.

98.61

8.93

7.13

0.40

n.a.

99.09

11
10

Cpx

52.06

0.54

1.77

10.55

0.34

14.45

20.18

0.48

n.d.

n.a.

100.38

Opx

53.12

0.32

1.34

18.60

0.46

24.45

1.30

0.02

n.d.

n.a.

99.61

10

Mt

n.a.

9.67

2.63

79.80

0.32

3.40

n.a.

n.a.

n.a.

0.83

96.67

11

Il

n.a.

38.00

0.57

55.17

0.23

3.80

n.a.

n.a.

n.a.

0.45

98.22

11

Gl matrix glass, Plg plagioclase, Am amphibole, Cpx clinopyroxene, Opx orthopyroxene, Mt titanomagnetite, Il ilmenite, n.a. not analyzed, n.d.
not detected, n number of analysis. 2 standard deviations for standards measured during the course of this study average 0.4 wt% Na2O, 0.1 wt%
Al2O3, 1 wt% SiO2, 0.1 wt% K2O, 0.2 wt% CaO, 0.6 wt% FeO, 0.5 wt% TiO2, 0.7 wt% MnO, 0.6 wt% MgO

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Page 5 of 19

966

Fig. 2 Total alkalis versus silica diagram for bulk-rock (solid

symbols) and groundmass glass (open symbols) compositions of the
Plinian deposits (Tables 1, 2). The shaded region outlines the field
defined by older lavas and tephra erupted since 1996 (Sosa-Ceballos
2006; Schaaf et al. 2005). Symbols are diamond WP, triangle GT, star
MT, pentagon OP, square LP, and circle PP

Fig. 3 Relative percentages of compositions of ca. 20 plagioclase c

crystals in each Popocatepetl Plinian magma (n = number of
analyses). For comparison, shaded area represents the distribution
of OP plagioclase

that a separate fluid was present throughout the run. We

first estimated the minimum amount of water needed from
the model of Papale et al. (2006), and then added more than
that to the capsule. The capsule was then weighed, welded
shut, heated on a hot plate, and weighed again to check for
leaks and ensure that no water was lost during welding. To
ensure that a fluid remained present throughout the run, the
capsule was weighted after quenching. In addition, when
the capsule was split open a slight hiss is heard if fluid is
present. Finally, fluid-saturated samples contain bubbles.
Equilibrium was approached by verifying the occurrence of
experimental phases and comparing the compositions of
experimental plagioclase within aliquots of previously run
material, one of which had run at a higher temperature and
the other at a lower temperature. MT, OP, and WP powders
were placed in separate, 2-mm-diameter Ag70Pd30 capsules, which were only crimped shut and placed inside a
5-mm-diameter Ag70Pd30 capsule to ensure previously run
materials equilibrated at the same pressure and temperature. Oxygen fugacity was buffered near that of the NiNiO
buffer reaction by using a Ni filler rod and water as the
pressurizing medium (Geschwind and Rutherford 1992;
Gardner et al. 1995a, b).
For experiments in TZM pressure vessels, 2-mm-diameter Ag70Pd30 capsules were welded at one end, powder
was added, and the capsule was crimped shut. Another
2-mm-diameter Ag70Pd30 capsule was welded at one end

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Contrib Mineral Petrol (2014) 167:966

Table 3 Textures and compositional variability in plagioclase

Texture 1 (%)

Texture 2 (%)

Texture 3 (%)

Texture 4 (%)

?D An (mol%)

-D An (mol%)

Plag affected (%)

WP

41

59

MT

86

14

14

24

14

32

30

GT

100

46

n.a.

n.a.

n.a.

OP

31

65

LP

19

31

50

14

16

27

22

25

36

Texture 1 = undisturbed zoned plagioclase; texture 2 = patchy sieved cores overgrown by undisturbed zoned plagioclase; texture 3 = zoned
plagioclase with sieved zones near the rim; texture 4 = thoroughly sieved crystals. DAn = maximum compositional variation (? positive,
- negative). Plag affected = percentage of crystal affected by compositional variations greater than 10 An mol% (taking the length of all
crystals from each eruption as 100 %)

Fig. 4 Back-scattered electron

images of representative
plagioclase crystals.
a oscillatory growth with
normal compositional zonation
(Group I), b patchy cores and
oscillatory growths (Group II),
c sieved zones near the rims
(Group III), and d thoroughly
sieved crystals (Group IV).
Scale bar is 250 lm in all
photos

and loaded with Ni metal and NiO powder and crimped

shut. Both capsules were then placed inside a 5-mmdiameter Ag70Pd30 capsule that contained enough distilled
water to both saturate the sample and facilitate the reaction
between the buffer materials. The 5-mm capsule was
welded shut and checked for leaks. The pressurizing
medium in the TZM pressure vessels was argon, to which
several bars of methane were added to maintain hydrogen
fugacity during the experiment to discourage hydrogen loss
from the capsule (Sisson and Grove 1993). At the end of
each run, the buffer and water were checked to ensure that

123

both Ni metal and NiO powder were still present and that
the experiment was water saturated. If one was absent, the
sample was discarded.

Results
All Plinian magmas are calk-alkaline, high-silica andesites,
except WP, which is a dacite (Table 1). Phenocryst contents
range from 13 to 36 vol% and consist of plagioclase, orthopyroxene, clinopyroxene, titanomagnetite, ilmenite, and

Contrib Mineral Petrol (2014) 167:966

Fig. 5 Distribution of Mg# ((Mg/Mg ? Fetot) 9 100) in orthopyroxene (opx) and clinopyroxene (cpx) from all Plinian magmas. Solid
bars are relatively Mg-rich pyroxenes in MT, LP, and PP, thought to
be most likely xenocrysts. Open bars are relatively Fe-rich pyroxenes
from all Plinian magmas

trace amounts of apatite and pyrrhotite, all set in vesicular

glass with abundant microlites of plagioclase and pyroxene.
Amphibole also occurs as phenocrysts and microlites in WP
and GT pumices. Matrix glass ranges in composition from
andesitic (MT) to rhyolitic (WP) (Fig. 2).
Plagioclase
Plagioclase phenocrysts range in size from about
1002,000 lm, and in composition from *An30 to *An60
with modes differing between magmas (Fig. 3). Plagioclase is unimodal in composition in OP and WP and
bimodal in LP, PP, and MT. The outer rims of plagioclase
in OP have compositions that match that of the mode,
whereas rims in each of the other magmas are diverse and
encompass the entire compositional range found in that
magma.
Overall, plagioclase can be grouped into four main
textural groups (Table 3). The first (Group I) consists of
crystals characterized by variably zoned compositions,
with only minor internal resorption boundaries and small

Page 7 of 19

966

glass inclusions (Fig. 4a). Most Group I crystals in WP and

OP are normally zoned from *An55 to *An40. A few in
WP are reversely zoned near their rims, increasing to
*An50. Group I crystals in LP and PP are more variable in
composition and are not consistently zoned between core
and rim.
The second group of plagioclase (Group II) consists of
crystals that have prominent patchy sieved cores that are
overgrown by plagioclase with only minor internal disturbances (Fig. 4b). The compositional difference between
cores and overgrowths is generally less than 15 mol%
anorthite, with cores being more anorthitic, except in PP in
which cores are more albitic (Table 3). Overgrowths on
Group II crystals in WP and OP are normally zoned with
compositions that match those from Group I. Most overgrowths in LP are unzoned, although a few are normally
zoned, decreasing from *An47 to *An37. Overgrowths on
PP crystals are reversely zoned from *An38 to *An52.
Group III plagioclase is similar to Group II, except that
there are prominent sieved zones near their rims (Fig. 4c).
Those outer sieve zones in MT, LP, and PP consist of
intricate networks of micron-sized glass inclusions that are
generally overgrown by up to 15 lm of texturally undisturbed plagioclase. Those outer growths are always more
albitic by 15 and 30 mol%. Two sieve zones occur close to
the rims of OP crystals, with the outer one characterized by
multiple melt inclusions (tens of microns in size) that are
often connected to the adjacent matrix glass.
The fourth group (Group IV) is thoroughly sieved
crystals with compositions of *An75 (Fig. 4d). A few of
those are mantled by micron-thick rims of unaltered plagioclase with compositions of *An50. Group IV crystals
are found only in GT.
Mafic minerals
Orthopyroxene and clinopyroxene occur in all deposits as
euhedral to subhedral phenocrysts up to 3,000 lm in size.
Orthopyroxene varies in composition between En65 and
Mg
 100).
En70, with Mg# = 5460 (where Mg# MgFe
total
Clinopyroxene varies between En39Fs20Wo41 and
En48Fs8Wo44, with Mg# = 5264. Both pyroxene types in
WP and OP lack internal disequilibrium textures and are
compositionally homogeneous. Pyroxenes in LP and PP are
texturally more diverse, with some having internal dissolution features. Amphibole occurs as phenocrysts in WP and
GT. Crystals in these magmas are compositionally homogeneous pargasite (Table 2). All are euhedral and lack
reaction rims.
Ilmenite and titanomagnetite, typically 525 lm in size,
occur in all magmas as compositionally unzoned crystals.
Ilmenite is more abundant, except in MT, and varies in

123

966 Page 8 of 19

Contrib Mineral Petrol (2014) 167:966

Table 4 Sr and Nd isotopic compositions

87

143

eNd

206

207

208

Gl

0.70458

0.51281

3.3

18.69

15.60

38.48

Plg

0.70444

0.51283

3.8

18.68

15.60

38.46

Cpx

0.70455

0.51282

3.5

18.67

15.58

38.41

Gl

0.70420

0.51285

4.1

18.65

15.61

38.44

Plg

0.70440

0.51282

3.5

18.68

15.56

38.30

Cpx

0.70421

0.51285

4.2

18.63

15.58

38.36

Gl

0.70445

0.51282

3.5

18.63

15.57

38.33

Plg
Cpx

0.70448
0.70449

0.51282
0.51283

3.5
3.8

18.63
18.65

15.56
15.59

38.32
38.41

Gl

0.70416

0.51286

4.4

18.65

15.60

38.43

Plg

0.70409

0.51286

4.3

18.63

15.58

38.35

Cpx

0.70415

0.51287

4.5

18.65

15.61

38.44

Gl

0.70430

0.51284

3.9

18.66

15.59

38.42

Plg

0.70429

0.51282

3.6

18.66

15.60

38.45

Cpx

0.70429

0.51284

3.9

18.63

15.56

38.31

Gl

0.70454

0.51283

3.8

18.68

15.61

38.48

Plg

0.70452

0.51282

3.6

18.66

15.60

38.45

Cpx

0.70452

0.51284

3.9

18.66

15.58

38.40

Eruption

Sr/86Sr

Nd/144Nd

Pb/204Pb

Pb/204Pb

Pb/204Pb

WP

MT

GT

OP

LP

PP

Gl matrix glass, Plg plagioclase, Cpx clinopyroxene. Total blanks for these procedures were 40 pg for Sr, 60 pg for Nd, and 16 pg for Pb. Sr data
are fractionation corrected to 88Sr/86Sr = 8.3752. 87Sr/86Sr ratios for NBS 987 measured during the course of this study average
0.710256 0.000005 (2 SD, n = 600). The Nd data are fractionation corrected to 146Nd/144Nd = 0.7219. 143Nd/144Nd ratios for La Jolla
standard measured during the course of this study average 0.511835 0.000005 (2 SD, n = 600)
The Pb data were corrected for *1.1 % amu-1 mass fractionation determined from the difference between the average measured values of NBS
981 Pb and the values 206Pb/207Pb = 0.9149, 206Pb/204Pb = 16.9418, 207Pb/204Pb = 15.5000, 208Pb/204Pb = 36.7265 reported for the same
standard in Baker et al. (2004). 206Pb/204Pb, 207Pb/204Pb, 208Pb/204Pb ratios and 2 standard deviations for NBS 981 measured during the course of
this study average 16.9031 0.006, 15.4466 0.008, and 36.5582 0.024, respectively

composition from Ilm63 to Ilm86. Titanomagnetite varies

from Usp20 to Usp70. Most magmas contain a single
compositional population of each (Table 2). Pre-eruptive
temperatures and oxygen fugacities of magmas were calculated using compositions of coexisting titanomagnetite
and ilmenite (Ghiorso and Evans 2008). Equilibrium
between titanomagnetite and ilmenite was confirmed using
the model of Bacon and Hirschmann (1988). In addition,
temperatures were estimated for WP and GT from compositions of amphibole phenocrysts (Ridolfi et al. 2010).
Differences between temperatures estimated from FeTi
oxides and amphibole are within uncertainties of the
models. Overall, temperature ranges from 875 15 to
960 20 C, and oxygen fugacities range from 0.7 to 1.3
log units above the NiNiO oxygen (NNO) buffer (Fig. 1).
There are no systematic changes in temperature with either
bulk composition or age.

123

Xenocrysts
Xenocrysts are found in most Plinian magmas and include
olivine (in MT, OP, LP, and PP), Cr-rich magnetite and
ilmenite (MT, LP), enstatite (MT, GT, LP, PP), barite (PP),
amphibole (MT), and calcic plagioclase (MT). Olivine in
MT, OP, LP, and PP contains reaction rims. Schaaf et al.
(2005) report olivine in the Popocatepetl magmas with
chromite inclusions, compositions between Fo70 and Fo90,
and orthopyroxene rims on Fo-rich olivine (MT and PP
magmas). They explain the reaction rims and the compositional range of olivine as a result of re-equilibration at
variable temperatures produced by mixing between mafic
and silicic magmas. Given the composition of the MT
groundmass (Table 2) and the Fo90 reported in Schaaf et al.
(2005), that would imply an ironmagnesium partition
coefficient (KFeMg
Dolivine-melt) of *0.10. Such a small value

Contrib Mineral Petrol (2014) 167:966

Page 9 of 19

966

Table 5 Experiments with MT, OP, and WP powders

Experiment

Material

Duration (h)

P (Mpa)

T (Celsius)

Run product phases

MT-5

Powder

96

50

900

MT-9

From MT-2

312

75

800

G, Plg, Pyx, Ox

MT-16

Powder

146

75

1,000

G, Plg, Pyx, Ox

MT-21

From MT-9

171

75

850

G, Plg, Pyx, Ox

MT-22

From MT-16

171

75

850

G, Plg, Pyx, Ox

MT-6

From MT-2

84

100

900

G, Plg, Pyx, Ox

MT-7

From MT-5

96

100

900

G, Plg, Pyx, Ox

MT-11

From MT-2

218

100

800

MT-18

From MT-16

96

100

1,000

MT-19

From MT-17

96

100

1,000

G, Plg, Pyx, Ox

MT-31
MT-8

Powder
From MT-5

96
96

100
125

1,150
900

G
G, Plg, Pyx, Ox

MT-10

From MT-1

103

125

900

G, Plg, Pyx, Ox

MT-12

From MT-2

219

125

800

G, Plg, Pyx, Ox, A

MT-17

Powder

96

125

1,000

MT-27a

From MT-2

168

125

850

MT-27b

From MT-1

168

125

850

G, Plg, Pyx, Ox, A

MT-1

Powder

96

150

900

G, Plg, Pyx, Ox, A

MT-2

Powder

168

150

800

G, Plg, Pyx, Ox, A

MT-28a

From MT-2

168

150

850

G, Plg, Pyx, Ox, A

MT-28b

From MT-1

168

150

850

G, Plg, Pyx, Ox, A

MT-26

From MT-2

168

175

825

G, Plg, Pyx, Ox, A, Bi

MT-3

From MT-1

96

200

875

G, Pyx, Ox, A

MT-4

From MT-2

169

200

825

MT-23

Powder

72

200

1,000

G, Pyx,

MT-24

From MT-23

96

200

975

G, Pyx,

MT-25
MT-29

From MT-23
From MT-25

72
144

200
200

925
850

G, Plg, Pyx, A
G, Plg, Pyx, Ox, A, Bi

MT-14

From MT-13

98

225

850

G, Pyx, Ox, A, Bi

MT-13

Powder

96

250

850

G, Pyx, Ox, A, Bi

OP-7

From OP-6

168

75

875

G, Plg, Pyx, Ox

OP-9

Powder

96

75

950

G, Plg, Pyx, Ox

OP-3

From OP-1

96

125

900

G, Plg, Pyx, Ox

OP-10

From OP-1

96

150

950

G, Pyx, Ox

OP-2

From OP-1

96

175

825

G, Plg, Pyx, Ox, A, Bi

OP-4

From OP-1

168

175

825

G, Plg, Pyx, Ox, A, Bi

OP-6

From OP-4

85

175

900

G, Pyx, Ox, A

OP-8

From OP-1

144

225

850

G, Pyx, Ox, A, Bi

OP-1

Powder

144

250

850

G, Pyx, Ox, A, Bi

WP-3

From WP-1

144

75

875

G, Plg, Pyx, Ox

WP-2

From WP-1

144

125

915

G, Plg, Pyx, Ox, A

WP-5
WP-4

From WP-1
From WP-1

144
144

175
225

900
850

G, Pyx, Ox, A, Bi
G, Pyx, Ox, A, Bi

WP-1

Powder

169

250

850

G, Pyx, Ox, A, Bi

G, Plg, Pyx, Ox

G, Plg, Pyx, Ox, A

G, Plg, Pyx, Ox

G, Pyx, Ox
G, Plg, Pyx, Ox, A

G, Plg, Pyx, Ox, A, Bi

G glass, Plg plagioclase, Pyx pyroxene, Ox opaque, FeTi oxides, A amphibole, Bi biotite, Powder initial material

indicates that those olivines are xenocrystic, and not in

equilibrium with the MT magma (e.g., Takahashi 1987).
Water-saturated experiments using magmas with similar

bulk composition to MT and LP, at similar fO2 conditions

(*log-10 fO2) but with greater concentrations of Cr and
Ni, grow olivine at 200 MPa and 1,000 C (Blatter and

123

966 Page 10 of 19

Carmichael 2001). We found, however, that experiments

using MT, OP, and WP pumice do not grow olivine at
those PT conditions.
Sosa-Ceballos et al. (2012) identified two populations of
pyroxenes in GT and MT magmas that resulted from mixing.
Very similar populations are found in LP and PP, with the
distinctly magnesian-rich pyroxenes considered xenocrystic
(Fig. 5). Amphibole and calcic plagioclase are also present
in MT, but Sosa-Ceballos et al. (2012) demonstrated that
those were inherited from GT and mafic magma, respectively, just before eruption. All Cr-rich ilmenites and titanomagnetites and those with exsolution textures in GT and
MT are related either to more mafic magma or to rocks
hosting the reservoir (Sosa-Ceballos et al. 2012). LP also
contains two compositional groups of FeTi oxides, one of
which consists of Cr-rich ilmenite and titanomagnetite that
may have equilibrated at *1,000 C and are considered
xenocrystic (Table 2). Barite was found in PP, which has not
been reported before in Popocatepetl magmas, and did not
grow experimentally; barite is thus considered xenocrystic.
Sr, Nd, and Pb isotopes
Matrix glasses vary in 87Sr/86Sr from 0.70416 to 0.70458, in
eNd from ?3.3 to ?4.4, in 206Pb/204Pb from 18.63 to 18.69,
in 207Pb/204Pb from 15.56 to 15.62, and in 208Pb/204Pb from
38.33 to 38.49 (Table 4). WP has the most radiogenic glass
in terms of Sr, whereas OP glass is least radiogenic. The
most radiogenic for Pb is MT, and the least is GT.
Plagioclase and clinopyroxene have variable Sr, Nd, and
Pb isotopic compositions (Table 4). In the case of plagioclases, the most radiogenic occur in PP, whereas the
most radiogenic clinopyroxenes occur in WP. The least
radiogenic crystals are both from OP. Clinopyroxenes are
in Sr, Nd, and Pb isotopic equilibrium with matrix glasses
for all eruptions, whereas plagioclases from MT and WP
are in isotopic disequilibrium with corresponding matrix
glasses and clinopyroxenes. The Pb isotopes for pyroxenes
in WP, GT, LP, and PP are in disequilibrium with plagioclase and groundmass, OP contains plagioclase in disequilibrium with pyroxene and groundmass, and in MT, all
3 phases are in disequilibrium. Overall, there is isotopic
disequilibrium between phases in all magmas.

Experimental results
Experiments were carried out using OP, MT, and WP
whole-rock samples between 800 and 1,050 C and 50 and
250 MPa. Although groundmass glass and many crystals in
MT are not in equilibrium, we used it as a proxy for
magmas of similar bulk composition with the assumption
that imparting a specific pressure and temperature on its

123

Contrib Mineral Petrol (2014) 167:966

bulk composition will yield a given mineral assemblage

and compositions (e.g., Gardner et al. 1995a, b). In fact,
compositions of experimentally produced plagioclase and
glass using MT coincide closely with those using OP,
which is similar in bulk composition to MT (Fig. 2),
demonstrating that the presence of disequilibrium phenocrysts, which comprises [30 vol% in MT, made little
difference. All experiments were run at pressures and
temperatures where melt and fluid (bubbles) were present
(Table 5). At 125 MPa, pyroxene and FeTi oxides are the
liquidus phases at *1,025 C, plagioclase appears at
*975 C, and amphibole at *900 C (Fig. 6). At
200 MPa, pyroxene crystallizes first at *1,000 C, then
amphibole at *950 C, FeTi oxides and biotite at
*875 C, and plagioclase at *800 C (Fig. 6).
Glass and crystals in experiments using MT and OP vary
similarly in composition with changes in water experimental pressure (75250 MPa) and temperature
(825950 C), although compositions in OP are slightly
more evolved at any given temperature and water pressure
(Table 6). In general, lower temperature and lower water
pressure result in more silicic melts that are enriched in
K2O and depleted in FeO, MgO, and CaO. Plagioclase also
varies in composition with water pressure and temperature
and, in general, becomes more albitic with decreasing

Fig. 6 Experimental results using OP (solid half symbols), MT (open

symbols), and WP (asterisk) samples. All experiments were water
saturated (PH2O = Ptotal) and run at an oxygen fugacity equal to or
slightly more oxidized than the NiNiO buffer curve. Glass (melt) and
vapor are present at all conditions. For MT runs, left-pointing arrows
represent crystallization experiments; right-pointing arrows, melting.
Squares represent natural powder run directly at those conditions.
Curves represent the upper stability limits for mineral phases (dashed
where inferred). Experimental plagioclase compositions are shown by
dotted curves, based on results from the MT runs. Results using OP
and WP samples generally match those of the MT runs

Contrib Mineral Petrol (2014) 167:966

Page 11 of 19

966

Table 6 Composition of experimental products

Experiment

MT-5

P (Mpa)

500

Na2O
(wt%)

T Celsius

900

MgO
(wt%)

Al2O3
(wt%)

SiO2
(wt%)

K2O
(wt%)

1.32

18.05

63.96

2.15

4.85

23.50

58.31

0.80

8.08

13.70
16.75

68.53
64.96

3.85
2.28

1.68
4.18

4.77

Plg

5.56
3.26
4.45

0.37
0.92

CaO
(wt%)

TiO2
(wt%)

MnO
(wt%)

0.54

0.06

2.29

98.00

0.96

97.21

1.20
2.09

92.83
96.35

750
750

800
1,000

G
G
Am

0.93

14.12

5.52

54.51

0.66

15.52

0.67

0.27

5.31

97.51

MT-22

750

850

3.28

0.29

12.42

69.93

3.50

1.27

0.31

0.03

1.31

92.34

MT-18

1,000

1,000

0.76

0.65

0.10

MT-31
MT-8

100

1,150

1,250

900

5.97
3.88

4.14

3.55
0.66

3.76

Plg

4.54

0.02
0.06

Oxide
Totals
(wt%)

MT-9
MT-16

Plg

0.23
0.66

FeO
(wt%)

15.44

67.15

2.75

2.41

30.21

51.99

0.14

13.20

16.34

57.19

1.76

5.72

0.73

0.11

0.46

0.06

14.34

64.09

2.69

2.55

25.09

60.20

0.65

8.49

1.83

97.08

0.31

99.74

5.00

94.54

2.29

90.90

0.89

99.86
91.30

MT-12

1,250

800

2.60

0.24

12.57

69.87

3.01

1.29

0.25

0.04

1.42

MT-17

1,250

1,000

5.04

2.23

17.34

59.54

1.62

5.51

0.77

0.09

4.63

96.76

MT-27a

1,250

850

3.57

0.30

13.86

70.18

3.08

1.47

0.30

0.03

1.52

94.33

MT-1

1,500

900

0.57

0.44

0.07

4.03

Plg

4.54

Am

2.75

G
Plg

4.17
6.12

15.05

64.50

2.55

2.60

25.68

57.28

0.57

9.53

5.42

14.41

57.24

1.57

5.94

0.80

0.45

18.03
23.74

62.46
61.74

2.00
0.69

4.51
6.75

0.43

2.38

92.18

0.74

98.34

0.17

5.85

94.14

0.01

2.26
0.60

94.32
99.63

MT-2

1,500

800

Am

3.00

3.29

15.51

60.88

1.63

4.98

0.38

0.09

2.93

92.69

MT-28a

1,500

850

3.47

0.47

14.21

69.06

2.95

1.76

0.27

0.03

1.36

93.57

MT-3

2,000

875

3.45

0.54

15.17

64.89

2.40

2.54

0.33

0.08

1.25

90.66

Am

2.38

10.08

12.29

51.25

1.18

7.56

1.29

0.20

7.05

93.27

0.27

0.08

0.02

MT-4

2,000

825

3.50

Plg

6.08

18.19

64.51

1.93

4.65

24.94

57.83

0.52

8.38

1.21

94.37

0.82

98.56

Am

2.05

11.64

11.18

52.03

0.78

8.68

1.23

0.25

9.27

97.11

MT-24

2,000

980

4.53

2.53

16.79

57.20

1.46

5.85

0.75

0.09

4.43

93.64

MT-25

2,000

925

4.30

0.94

16.49

61.04

2.02

3.70

0.38

0.09

3.40

92.37

MT-29

2,000

850

3.46

0.48

15.17

67.24

2.49

1.97

0.30

0.05

1.35

92.50

MT-14

2,250

850

3.07

0.25

15.35

62.60

2.22

2.33

0.24

0.05

1.19

87.30

MT-13

2,500

850

2.80

0.49

16.11

64.66

2.08

2.34

0.33

0.07

1.37

90.24

750

875

3.81

0.63

14.32

71.02

3.38

0.94

0.32

0.04

1.24

95.71

OP-7
OP-9

750

950

3.90

0.83

15.33

66.77

2.87

1.90

0.64

0.06

3.02

95.31

OP-3
OP-10

1,250
1,500

900
950

G
G

4.14
4.37

1.03
1.21

15.71
15.71

66.69
62.55

2.84
2.47

1.96
2.34

0.54
0.40

0.09
0.07

1.95
1.32

94.95
90.43

OP-2

1,750

825

3.13

0.25

0.07

Plg
OP-4

1,750

825

3.45

Plg

0.46

14.13

69.05

2.72

1.31

6.22

26.36

57.81

0.58

8.77

0.61

14.24

67.83

2.43

1.47

6.30

24.67

60.24

0.57

7.10

0.28

0.07

1.33

92.46

0.60

100.41

1.34

91.71

0.45

99.33

OP-6

1,750

900

3.80

1.12

16.14

64.95

2.33

2.69

0.52

0.07

2.19

93.81

OP-8

2,250

850

3.57

0.89

15.23

66.01

2.20

2.34

0.29

0.07

1.52

92.12

OP-1

2,500

850

3.64

0.76

15.42

64.86

2.40

2.29

0.31

0.07

1.45

91.21

G glass, Plg plagioclase, Am amphibole, n.a. not analyzed

temperature and decreasing water pressure (Fig. 6). Overall, compositional variations of amphibole with changes of
pressure and temperature are more scattered, but in general,

Na2O, FeO, and MnO contents tend to be greater at lower

temperature. Pyroxene and biotite were identified by
morphology only and are too small to analyze.

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Contrib Mineral Petrol (2014) 167:966

Fig. 8 Maximum incremental increase in An contents in plagioclase

crystals from each Plinian deposit as a function of the percentage of
plagioclase affected by changes in An contents

Magma mixing

Fig. 7 Compositional transects of representative PP, LP, and MT

plagioclases. Solid bars represent crystal lengths affected by positive
increments of [5 mol%. Open bars represent lengths affected by
negative decrements [5 mol%. The ratio represents the total length
affected by positive increments divided by the total length of the
crystal

Discussion
The occurrence of dissolution features and compositional
fluctuations in plagioclase and pyroxenes, xenocrysts
(olivine, Cr-rich FeTi oxides, and Mg-rich pyroxenes), and
isotopic disequilibria between coexisting phases all indicate
that magma mixing has occurred repeatedly before each
Plinian eruption over the past *23 ky. But, how frequent
and how intense have those mixing events been? Also, if
mixing has repeatedly occurred, why have erupted magmas
remained relatively constant in composition and not tended
to become more mafic with time? In fact, the relatively
constant bulk composition suggests that injections of mafic
magma were either balanced by other processes that drive
bulk magma compositions back toward more silicic compositions, or of small enough magnitude to have been
insignificant relative to the pre-existing bulk magma.

123

According to textural and compositional evidence in plagioclase, mixing has been uneven between Popocatepetl
Plinian magmas. For example, the lack of sieving textures
in WP crystals and the wider range in compositions in MT
and PP plagioclase, which overall are more albitic than WP
crystals (Fig. 3), suggest magmas were modified by different amounts of mixing through time.
In order to investigate the intensity and frequency of
mixing events, we use the occurrence and magnitude of
compositional variations along traverses in plagioclase
from all magmas as proxies (an average of 20 crystals
each) (Table 3). We ignore GT plagioclase because the
abundant glass inclusions prevented measurement of
uninterrupted linear transects. Compositional variations are
either positive (increasing An mol%) or negative
(decreasing An mol%) and were measured over the length
of a crystal and normalized to the total length of that crystal
(Fig. 7). We focus on variations that occur within lengths
of less than 40 lm, because most sharp variations, where
composition changes by more than 10 An mol%, occur in
less than 40 lm. Changes spread out across more than
40 lm are almost always smooth decreases in An content.
Fluctuations of less than 5 mol% are ignored because such
differences are near analytical precision. The largest variations in An contents often exceed 10 mol% (Fig. 7).
Based on our experimental results, if changes in plagioclase composition by 10 mol% were to occur isothermally,

Contrib Mineral Petrol (2014) 167:966

Fig. 9 Frequency of mixing events recorded in plagioclase. Mixing

events (mafic injections) are based on the assumption that an increase
in An content of C10 mol% is produced by a mixing event. For
example, 5 % of crystals in MT and LP record more than 35 events in
a decade, yet 55 % of crystals in WP record fewer than 5 of such
events in the same time span. Years are estimated assuming a
plagioclase growth rate of 2.5 9 10-6 lm/s (Izbekov et al. 2002)

then water pressure would have had to change by more

than 125 MPa (Fig. 6). In other words, the crystal would
need to sink or float by 4 to 5 km. That seems far for
individual crystals to travel inside a magma, especially
considering many crystals have more than one of such

Page 13 of 19

966

fluctuation. Most of the compositional variability in plagioclase is thus assumed to result from changes in temperature and/or melt composition, that is from mixing
events.
Overall, the percentage of individual crystals affected by
positive and negative variations ranges from *5 to 97 %,
with a positive shift of 32 mol% An being the maximum
variation found. Individual crystals in MT have the greatest
variations in composition, whereas those in WP and OP are
the least variable. Overall, the greatest increases in An
content are found in Group III crystals (MT, LP, and PP),
whereas the smallest increases are found in Group I crystals (WP, OP). When lengths of fluctuations in composition
are summed for all crystals in a population and normalized
to the total length of all crystals measured in that population, it is found that MT plagioclase is, on average, the
most variable (Fig. 8). In contrast, plagioclase from WP
and OP is again the least variable, with only 2529 % of
the total measured length affected.
In order to investigate the frequency of significant mafic
injections, as represented by increases in An content of
C10 mol%, we convert our analyzed plagioclase transects
to equivalent time spans. We estimate time using plagioclase growth rates. Although plagioclase growth is unlikely
to be constant, because of changes in temperature and
water pressure, a general growth rate range has been estimated at 10-5 to 10-7 lm/s (e.g., Dowty 1980; Cashman
and Marsh 1988; Izbekov et al. 2002). For each crystal, the
total length of analyzed transect was converted into duration using a growth rate of 2.5 9 10-6 lm/s. Analyzed
transects thus represent between 2 and 20 years of crystallization. Those times must be viewed as minima,
because all crystals contain evidence of partial dissolution.
The number of compositional positive variations that
exceed 10 mol% An in each transect was then divided by
the amount of time represented by the transect, yielding
how frequent such large variations occur (Fig. 9). Not
surprisingly, the frequency of such events is variable. More
than 50 % of crystals in MT, LP, and PP preserve more
than 10 mafic injections every decade, whereas more than
90 % of crystals in OP and WP record less than 8 injections
every decade, and some even lack any evidence of mixing
(Fig. 9). Thus, some magmas had relatively long quiescent
periods (WP, OP), whereas others were modified frequently (MT, LP, PP). Most crystals have growth rims on
them, rather than dissolution rinds. If eruptions are triggered by mixing (e.g., Sparks et al. 1977), then the timescale of mixing was too short for it to be recorded.
Restoration of silicic compositions
Our evaluation suggests that some magmas erupted in
Plinian events experienced more numerous mixing events

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Contrib Mineral Petrol (2014) 167:966

Table 7 Input data for AFC models

DPb

eNd

0.70745

-0.52

17

0.70695

-3.65

0.707

-1.99

18.9031

17

0.704

5.5

18.6316

DSr

DNd

0.2

1.2

0.15

222

II

0.2

1.2

0.15

800

III

0.2

0.4

0.03

292

17

408

15

0.03

Parent magma

Sr

87

Model

Nd

Pb

Sr/86Sr

206

Pb/204Pb

r is the ratio of rate of assimilation to rate of crystallization

D is the bulk partition coefficient of Sr, Nd, and Pb
Nd, Sr, and Pb concentrations in ppm

(Fig. 8) and more frequent large ones (Fig. 9). Despite

variable frequency, bulk composition remained silicic and
temperatures do not correlate with frequency. If positive
An shifts reflect mixing, then the more frequent events
must have been either relatively small or balanced by other
processes occurring more frequently.
Interestingly, almost every large increase in An content
is followed by a decrease in similar magnitude, suggesting
that the two may be linked. Such a link could be related, for
example, to the mixing events triggering crustal assimilation (Andrews et al. 2008) or rapid cooling driving fractional crystallization. Major element variations can in fact
be modeled as a result of fractional crystallization of an
assemblage similar to the modal mineralogy seen, but
variations in isotopic compositions show that crystallization alone is insufficient.
Previous work has related relatively enriched Sr isotopic
ratios in Popocatepetl magmas to carbonate assimilation
(Siebe et al. 2004; Schaaf et al. 2005). We investigate the
relevance of assimilation and crystallization in the Plinian
magmas using the assimilation-fractional crystallization
(AFC) model of De Paolo (1981). For such modeling, we
consider a basaltic andesitic mafic scoria found in the 2001
Popocatepetl eruption as a potential parental magma. Plinian deposits do not contain mafic xenolith, and so the
scoria was used as a proxy end member for the magmatic
processes that might occurred in the past. Three crustal
assimilants were assumed: a sandstone xenolith (Schaaf
et al. 2005), a fine-grained skarn, and a coarse-grained
skarn (Sosa-Ceballos 2003). All crustal xenoliths were
collected from Popocatepetl Plinian deposits. Although
other xenoliths have been found (e.g., marbles, limestones,
intrusive rocks), sandstone and skarns were chosen because
of their relative abundance and representative composition.
Input parameters for AFC modeling (bulk distribution, D,
and ratios of rates of assimilation to crystallization, r) are
listed in Table 7.
Models using the coarse-grained skarn (Model III in
Table 7) can reproduce the observed variations in major
elements and Sr isotopes, when the rate of fractional
crystallization exceeds that of assimilation (0.2 \ r\0.5).

123

If crystallization greatly dominates (r B 0.2), however, the

isotopic variability of the magmas cannot be explained. On
the other hand, if assimilation were extensive (i.e.;
r C 0.5), bulk compositions would trend toward the skarn
composition, and not match those of magmas erupted in the
Plinian events (Fig. 10).
If minor amounts of assimilation contributed to the
evolution of the Plinian magmas, then all isotopic systems
should be modified similarly. Calculated AFC model trends
for SrNd isotopes using either the sandstone or the finegrained skarn (Models I and II) fail to account for variations of the data, regardless of input parameters (Fig. 11a).
Model III was calculated using the coarse-grained skarn.
With a rate of assimilation equal to half that of crystallization (r = 0.5) assimilation of the coarse-grained skarn
matches only the more radiogenic samples (Fig. 11a). If
fractional crystallization dominates (r B 0.2), the general
isotopic trend persists, but the amount of differentiation
required cannot explain the bulk compositions of magmas.
Pb-Sr isotopic variations also argue against skarn
assimilation (Fig. 11b). Indeed, Pb isotope mixing trends
should be linear, but regardless of the Pb isotopic composition of the mafic end member, Popocatepetl magma
compositions do not trend toward the skarn signature,
which has enriched 206Pb/204Pb values for given
208
Pb/204Pb and 207Pb/204Pb ratios (Fig. 12). Pb isotopes
thus suggest skarn assimilation could not have significantly
modified the composition of magmas.
Isotopic compositions of magmas erupted in Plinian
events thus imply that assimilation of local crustal rocks is
limited at most. Further support comes from comparing all
Popocatepetl magma compositions to those of two nearby
volcanic systems, Nevado de Toluca (NT) and Sierra
Chihinautzin volcanic filed (SCVF). Erupted products from
both NT and SCVF have similar variations in terms of Pb
isotopes as Popocatepetl magmas. But, Nevado de Toluca
does not overlie shallow carbonates, ruling out such
assimilation. SCVF does overlie carbonates, but those
magmas ascended to the surface with minimal stagnation in
the upper crust, and hence little carbonate assimilation
(Siebe et al. 2004; Hansen and Nielsen 1999). Therefore,

Contrib Mineral Petrol (2014) 167:966

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966

evidence of carbonate assimilation. But, the overall compositional variations indicate that the extent of carbonate
assimilation into Popocatepetl Plinian magmas was limited.
This suggests that magmas erupted in Plinian events at
Popocatepetl arrive into the upper crust differentiated by
fractional crystallization, and if assimilation does occur,
then crust different from the shallow calcareous basement
was involved. The Sr isotopic compositions of xenoliths
from the upper mantle and lower crust below central
Mexico range from 0.70309 to 0.7279 (Ruiz et al. 1988;
Schaaf et al. 1994). Partial assimilation of such rocks could
explain the observed variations in Popocatepetl magmas.
Alternatively, the compositional variability of Popocatepetl
Plinian magmas could result from mantle heterogeneity
(e.g., Luhr 1997; Meriggi et al. 2008; Straub et al. 2008;
Johnson et al. 2009). Indeed, the general trend of Pb isotopes from NT, SCVF, and Popocatepetl magmatic series
could be explained by variable contribution of subducted
sediments (Fig. 12). Generation of magmas from partial
melting of different portions of the mantle coupled with
variable degrees of fractional crystallization and assimilation of lower crust (e.g., Smith and Leeman 1987; Annen
et al. 2006; Ownby et al. 2010) could be important factors
contributing to the compositional variability of the Plinian
magmas from Popocatepetl.
Reconstruction of the magmatic plumbing system

Fig. 10 Variation in major-element compositions as a function of Sr

isotopic composition. Solid symbols are data from this study, open
symbols are data from either lavas younger than 300 ky (SosaCeballos 2006) or recent products (Schaaf et al. 2005). Curves are
calculated trends using AFC models (see Table 7), assuming endmember compositions of scoria collected from the pyroclastic flow
deposit erupted in 2001 (Schaaf et al. 2005) and a coarse-grained
skarn (Sosa-Ceballos 2006). Values of used r in the models are
shown. Tick marks along trends are the percentage crystallized

although Plinian magmas erupted from Popocatepetl contain evidence of mixing, it seems that such energy input did
not precipitate assimilation of carbonates.
The lack of major carbonate assimilation does not preclude assimilation altogether. Indeed, the occurrence of
partially digested carbonates found in some Popocatepetl
lavas (Siebe, personal communication) shows clear

Plinian eruptions of Popocatepetl tapped magma that is

either amphibole-bearing (WP, GT) or amphibole-free
(MT, OP, LP, PP). The presence of amphibole requires
relatively high water pressures, and hence deeper storage
(Rutherford et al. 1985, Gardner et al. 1995a, b). Indeed,
relatively high water pressures are required to stabilize
amphibole because pre-eruptive temperatures of amphibole-bearing WP and GT magmas exceed 900 C. We
found that experiments with WP at 900 C stabilize
amphibole only at water pressures greater to 125 MPa.
In addition, amphibole compositions in both GT and WP
are consistent with water pressures in excess of
200 MPa (Ridolfi et al. 2010). Finally, Holtz et al.
(2005) and Martel et al. (1999) performed experiments
on bulk compositions similar to that of GT and found
that water pressure must be at least 200 MPa to crystallize amphibole above 900 C. On the other hand,
experiments at high water pressures using MT, OP, and
WP grew biotite (Fig. 6), yet natural samples are biotite
free. The lack of biotite in natural samples constrains
storage to be less than *250 MPa.
For amphibole-free magmas, experimental results
equivalent to pre-eruptive temperatures indicate that an
assemblage of plagioclase ? two pyroxene ? FeTi oxides is stable only at water pressures below 110130 MPa

123

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Contrib Mineral Petrol (2014) 167:966

Fig. 11 a eNd, and b 206Pb204

/ Pb
versus 87Sr/86Sr isotopic data
for glass, plagioclase, and
pyroxene separates from
Popocatepetl Plinian deposits.
See Fig. 2 for symbols.
Representation of 2r standard
deviations are shown as cross
bars. Solid symbols are used
when all three phases are in
equilibrium, and open symbols
indicate one phase is out of
equilibrium (plagioclase in both
cases). Inset shows AFC models
using different xenoliths as
assimilants end members.
Values of r 0.2 and 0.5 are used
to delineate the most likely AFC
conditions observed in Fig. 11.
Model I = sandstone, Model
II = fine-grained skarn, Model
III = coarse-grained skarn
(Schaaf et al. 2005; SosaCeballos 2006). Compositions
of Nevado de Toluca (NT)
(Martnez-Serrano et al. 2004)
and cones from Sierra
Chichinautzin volcanic field
(SCVF) (Agustn-Flores et al.
2011) are shown for comparison

(Fig. 6). Compositions of plagioclase, which generally

fluctuate between An40 and An55, are consistent with such
relatively shallow storage (Fig. 6).
Magma mixing recorded in plagioclase must have thus
occurred in two storage regions over the past 23 ky. One of
those regions must have been within 200250 MPa and the
other shallower than 130 MPa. Magmas from both the deep
and shallow reservoirs were tapped during the 14 ka Plinian eruption. This indicates that the pressures recorded
reflect different depths in the magmatic system, and not
changes resulting from edifice collapse (Pinel et al. 2010).
The deeper reservoir was tapped during the two older
Plinian eruptions. Mixing between magmas was diverse in
that region, as plagioclase in WP records only a few such
events before that eruption. In contrast, plagioclase textures
and compositions suggest mixing was thorough before the
GT magma was erupted. The shallower reservoir was
tapped during the last four Plinian eruptions and, except for
OP, appears to be a zone of frequent mixing events
(Fig. 9).
The difference in storage depth also limits the likely
extent of carbonate assimilation. The two storage reservoirs
are separated by *70 MPa, or roughly about 2,600 m of

123

rock, assuming an average density of 2,500 kg/m3. The

thickness of the carbonate platform underneath Popocatepetl has been well constrained to between 250 and 1,000 m
(e.g., Fries 1960; Johnson 1990; Cabral-Cano et al. 2000).
This suggests that only one of the reservoirs could have
been hosted by limestone. The more likely candidate is the
shallower one, because OP and MT magmas contain
fragments of calcareous rocks (Arana-Salinas et al. 2010;
Sosa-Ceballos et al. 2012) and PP contains xenocrysts of
barite. The absence of calcareous xenoliths in WP and GT
magmas from the deeper reservoir is important, because
their isotopic signatures are similar to, and in some cases
more enriched than, magmas from the shallow reservoir
(Fig. 11). This suggests that either the deeper reservoir was
hosted by carbonate rocks of unknown age or the isotopic
composition of Popocatepetl Plinian magmas reflects processes unrelated to carbonate assimilation.

Conclusions
Plinian eruptions of Popocatepetl over the past
23,000 years have tapped magmas from two reservoirs, one

Contrib Mineral Petrol (2014) 167:966

Page 17 of 19

966

References

Fig. 12 Pb isotopic compositions for groundmass glass, plagioclase,

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